Engineering the magnetism of nanographene via co-depositing hetero precursors

Abstract The magnetism of carbon nanomaterials is dominated by the structure of its carbon skeleton. However, the magnetism engineering is hindered due to finite precursors. Here, we develop a new strategy to engineer the magnetism of nanographene through hetero-coupling two different precursors on Au(111) surface by using low-temperature bond-resolved scanning tunneling microscopy and scanning tunneling spectroscopy, combined with spin-polarized density functional theory calculations. Our results demonstrate that two homo-coupled products host close shell structure along with defects inducing magnetic one with the total spin number S = 1/2. Upon simultaneous depositing with another precursor, two hetero-coupled products switch to magnetic structure with the S = 1/2 and S = 1 resulting from carbon skeleton transformation. Our results provide a valid way via inducing different molecular precursors to engineer the magnetism of carbon nanomaterials, which could be extended in other magnetic materials instruction.